Hydrate Stability and Methane Recovery from Gas Hydrate through CH4–CO2 Replacement in Different Mass Transfer Scenarios

Abstract

CH4–CO2 replacement is a carbon-negative, safer gas production technique to produce methane gas from natural gas hydrate reservoirs by injecting pure CO2 or other gas mixtures containing CO2. Laboratory-scale experiments show that this technique produces low methane volume and has a slow replacement rate due to the mass transfer barrier created due to impermeable CO2 hydrate layer formation, thus making the process commercially unattractive. This mass-transfer barrier can be reduced through pressure reduction techniques and chemical techniques; however, very few studies have focused on depressurization-assisted and chemical-assisted CH4–CO2 replacement to lower mass-transfer barriers and there are many unknowns. In this work, we qualitatively and quantitatively investigated the effect of the pressure reduction and presence of a hydrate promoter on mixed hydrate stability, CH4 recovery, and risk of water production during CH4–CO2 exchange. Exchange experiments were carried out using the 500 ppm sodium dodecyl sulfate (SDS) solution inside a high-pressure stirred reactor. Our results indicated that mixed hydrate stability and methane recovery depends on the degree of pressure reduction, type, and composition of injected gas. Final selection between CO2 and CO2 + N2 gas depends on the tradeoff between mixed hydrate stability pressure and methane recovery. Hydrate morphology studies suggest that production of water during the CH4–CO2 exchange is a stochastic phenomenon that is dependent on many parameters.